Stable and solubilized active Au atom clusters for selective epoxidation of cis-cyclooctene with molecular oxygen

Qian, Linping; Wang, Zhen; Beletskiy, Evgeny V.; Liu, Jingyue; dos Santos, Haroldo J.; Li, Tiehu; Rangel, Maria do C.; Kung, Mayfair C.; Kung, Harold H.

doi:10.1038/ncomms14881

Title: Stable and solubilized active Au atom clusters for selective epoxidation of cis-cyclooctene with molecular oxygen

Journal Article · Tue Mar 28 00:00:00 EDT 2017 · Nature Communications

DOI:https://doi.org/10.1038/ncomms14881· OSTI ID:1361195

Qian, Linping ^[1]; Wang, Zhen ^[2]; Beletskiy, Evgeny V. ^[3]; Liu, Jingyue ^[4]; dos Santos, Haroldo J. ^[5]; Li, Tiehu ^[6]; Rangel, Maria do C. ^[7]; Kung, Mayfair C. ^[3];

^[3]

Fudan Univ., Shanghai (China); Northwestern Polytechnical Univ., Shaansi (China)
Northwestern Polytechnical Univ., Shaansi (China); Northwestern Univ., Evanston, IL (United States)
Northwestern Polytechnical Univ., Shaansi (China)
Arizona State Univ., Tempe, AZ (United States)
Northwestern Polytechnical Univ., Shaansi (China); Univ. Federal da Bahia, Bahia (Brazil); Ciencia e Tecnologica da Bahia, Bahia (Brazil)
Northwestern Univ., Evanston, IL (United States)
Univ. Federal da Bahia, Bahia (Brazil)

Here, the ability of Au catalysts to effect the challenging task of utilizing molecular oxygen for the selective epoxidation of cyclooctene is fascinating. Although supported nanometre-size Au particles are poorly active, here we show that solubilized atomic Au clusters, present in ng ml^–1 concentrations and stabilized by ligands derived from the oxidized hydrocarbon products, are active. They can be formed from various Au sources. They generate initiators and propagators to trigger the onset of the auto-oxidation reaction with an apparent turnover frequency of 440 s^–1, and continue to generate additional initiators throughout the auto-oxidation cycle without direct participation in the cycle. Spectroscopic characterization suggests that 7–8 atom clusters are effective catalytically. Extension of work based on these understandings leads to the demonstration that these Au clusters are also effective in selective oxidation of cyclohexene, and that solubilized Pt clusters are also capable of generating initiators for cyclooctene epoxidation.

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Research Organization:: Northwestern Polytechnical Univ., Shaansi (China)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: FG02-03ER15457

OSTI ID:: 1361195

Journal Information:: Nature Communications, Vol. 8; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 32 works

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